Showing papers by "Jiwoong Park published in 2019"

Wafer-scale synthesis of monolayer two-dimensional porphyrin polymers for hybrid superlattices

Abstract: The large-scale synthesis of high-quality thin films with extensive tunability derived from molecular building blocks will advance the development of artificial solids with designed functionalities. We report the synthesis of two-dimensional (2D) porphyrin polymer films with wafer-scale homogeneity in the ultimate limit of monolayer thickness by growing films at a sharp pentane/water interface, which allows the fabrication of their hybrid superlattices. Laminar assembly polymerization of porphyrin monomers could form monolayers of metal-organic frameworks with Cu2+ linkers or covalent organic frameworks with terephthalaldehyde linkers. Both the lattice structures and optical properties of these 2D films were directly controlled by the molecular monomers and polymerization chemistries. The 2D polymers were used to fabricate arrays of hybrid superlattices with molybdenum disulfide that could be used in electrical capacitors.

Stacking angle-tunable photoluminescence from interlayer exciton states in twisted bilayer graphene.

Abstract: Twisted bilayer graphene (tBLG) is a metallic material with two degenerate van Hove singularity transitions that can rehybridize to form interlayer exciton states. Here we report photoluminescence (PL) emission from tBLG after resonant 2-photon excitation, which tunes with the interlayer stacking angle, θ. We spatially image individual tBLG domains at room-temperature and show a five-fold resonant PL-enhancement over the background hot-electron emission. Prior theory predicts that interlayer orbitals mix to create 2-photon-accessible strongly-bound (~0.7 eV) exciton and continuum-edge states, which we observe as two spectral peaks in both PL excitation and excited-state absorption spectra. This peak splitting provides independent estimates of the exciton binding energy which scales from 0.5–0.7 eV with θ = 7.5° to 16.5°. A predicted vanishing exciton-continuum coupling strength helps explain both the weak resonant PL and the slower 1 ps−1 exciton relaxation rate observed. This hybrid metal-exciton behavior electron thermalization and PL emission are tunable with stacking angle for potential enhancements in optoelectronic and fast-photosensing graphene-based applications. Interlayer electronic states in twisted bilayer graphene are characterized by flat-band regions hosting many-body electronic effects. Here, the authors observe two-photon photoluminescence excitation and excited-state absorption spectra on graphene containing a variety of twist angles to access the dark exciton transitions and estimate the exciton binding energy.

Reversible MoS2 Origami with Spatially Resolved and Reconfigurable Photosensitivity.

Abstract: Two-dimensional layered materials (2DLMs) have been extensively studied in a variety of planar optoelectronic devices. Three-dimensional (3D) optoelectronic structures offer unique advantages inclu...

Two-Dimensional Material Tunnel Barrier for Josephson Junctions and Superconducting Qubits

Abstract: Quantum computing based on superconducting qubits requires the understanding and control of the materials, device architecture, and operation. However, the materials for the central circuit element, the Josephson junction, have mostly been focused on using the AlOx tunnel barrier. Here, we demonstrate Josephson junctions and superconducting qubits employing two-dimensional materials as the tunnel barrier. We batch-fabricate and design the critical Josephson current of these devices via layer-by-layer stacking N layers of MoS2 on the large scale. Based on such junctions, MoS2 transmon qubits are engineered and characterized in a bulk superconducting microwave resonator for the first time. Our work allows Josephson junctions to access the diverse material properties of two-dimensional materials that include a wide range of electrical and magnetic properties, which can be used to study the effects of different material properties in superconducting qubits and to engineer novel quantum circuit elements in the future.

Capillary Origami with Atomically Thin Membranes

Abstract: Small-scale optical and mechanical components and machines require control over three-dimensional structure at the microscale. Inspired by the analogy between paper and two-dimensional materials, origami-style folding of atomically thin materials offers a promising approach for making microscale structures from the thinnest possible sheets. In this Letter, we show that a monolayer of molybdenum disulfide (MoS2) can be folded into three-dimensional shapes by a technique called capillary origami, in which the surface tension of a droplet drives the folding of a thin sheet. We define shape nets by patterning rigid metal panels connected by MoS2 hinges, allowing us to fold micron-scale polyhedrons. Finally, we demonstrate that these shapes can be folded in parallel without the use of micropipettes or microfluidics by means of a microemulsion of droplets that dissolves into the bulk solution to drive folding. These results demonstrate controllable folding of the thinnest possible materials using capillary origami and indicate a route forward for design and parallel fabrication of more complex three-dimensional micron-scale structures and machines.

Stacking, strain, and twist in 2D materials quantified by 3D electron diffraction

Abstract: The field of two-dimensional (2D) materials has expanded to multilayered systems in which electronic, optical, and mechanical properties change---often dramatically---with stacking order, thickness, twist, and interlayer spacing. For transition metal dichalcogenides (TMDs), bond coordination within a single van der Waals layer changes the out-of-plane symmetry that can cause metal-insulator transitions or emergent quantum behavior. Discerning these structural order parameters is often difficult using real-space measurements; however, we show that 2D materials have distinct, conspicuous three-dimensional (3D) structure in reciprocal space described by nearly infinite oscillating Bragg rods. Combining electron diffraction and specimen tilt we probe Bragg rods in all three dimensions to identify multilayer structure with subangstrom precision across several 2D materials---including TMDs (${\mathrm{MoS}}_{2}$, ${\mathrm{TaSe}}_{2}$, ${\mathrm{TaS}}_{2}$) and multilayer graphene. We demonstrate quantitative determination of key structural parameters such as surface roughness, inter- and intralayer spacings, stacking order, and interlayer twist using a rudimentary transmission electron microscope. We accurately characterize the full interlayer stacking order of multilayer graphene (1, 2, 6, 12 layers) as well the intralayer structure of ${\mathrm{MoS}}_{2}$ and extract a chalcogen-chalcogen layer spacing of $3.07\ifmmode\pm\else\textpm\fi{}0.11$ \AA{}. Furthermore, we demonstrate quick identification of multilayer rhombohedral graphene.

Twist, slip, and circular dichroism in bilayer graphene

Abstract: Stacking atomically thin two-dimensional materials with a rotational misalignment between their layers produces a van der Waals bilayer in which all mirror symmetries can be broken. A fundamental experimental signature of a twisted multilayer is circular dichroism (CD): the conversion of a linearly polarized incident optical field to an elliptically polarized field in transmission. This work investigates the relations between CD, the twist angle, and interlayer slip. In experiments where bilayers are formed by contacting one layer with another, the relative rotation angle between the symmetry axes of each sheet are controlled, but the lateral shifts between the layers are not. Accounting for the lateral shift between the layers expands the configuration space of twisted bilayer structures. Here we demonstrate how the symmetry constraints in this expanded configuration space are expressed in the CD spectrum of twisted bilayer graphene as a function of the rotation angle and interlayer slip.

Stacking, Strain, & Twist in 2D Materials Quantified by 3D Electron Diffraction

Abstract: The field of two-dimensional (2D) materials has expanded to multilayered systems where electronic, optical, and mechanical properties change-often dramatically-with stacking order, thickness, twist, and interlayer spacing [1-5]. For transition metal dichalcogenides (TMDs), bond coordination within a single van der Waals layer changes the out-of-plane symmetry that can cause metal-insulator transitions [1, 6] or emergent quantum behavior [7]. Discerning these structural order parameters is often difficult using real-space measurements, however, we show 2D materials have distinct, conspicuous three-dimensional (3D) structure in reciprocal space described by near infinite oscillating Bragg rods. Combining electron diffraction and specimen tilt we probe Bragg rods in all three dimensions to identify multilayer structure with sub-Angstrom precision across several 2D materials-including TMDs (MoS2, TaSe2, TaS2) and multilayer graphene. We demonstrate quantitative determination of key structural parameters such as surface roughness, inter- & intra-layer spacings, stacking order, and interlayer twist using a rudimentary transmission electron microscope (TEM). We accurately characterize the full interlayer stacking order of multilayer graphene (1-, 2-, 6-, 12-layers) as well the intralayer structure of MoS2 and extract a chalcogen-chalcogen layer spacing of 3.07 +/- 0.11 Angstrom. Furthermore, we demonstrate quick identification of multilayer rhombohedral graphene.

MoS2 pixel arrays for real-time photoluminescence imaging of redox molecules.

Abstract: Measuring the behavior of redox-active molecules in space and time is crucial for understanding chemical and biological systems and for developing new technologies. Optical schemes are noninvasive and scalable, but usually have a slow response compared to electrical detection methods. Furthermore, many fluorescent molecules for redox detection degrade in brightness over long exposure times. Here, we show that the photoluminescence of “pixel” arrays of monolayer MoS2 can image spatial and temporal changes in redox molecule concentration. Because of the strong dependence of MoS2 photoluminescence on doping, changes in the local chemical potential substantially modulate the photoluminescence of MoS2, with a sensitivity of 0.9 mV / Hz on a 5 μm × 5 μm pixel, corresponding to better than parts-per-hundred changes in redox molecule concentration down to nanomolar concentrations at 100-ms frame rates. This provides a new strategy for visualizing chemical reactions and biomolecules with a two-dimensional material screen.

MoS$_{2}$ pixel arrays for real-time photoluminescence imaging of redox molecules.

Abstract: Measuring the behavior of redox-active molecules in space and time is crucial for better understanding of chemical and biological systems and for the development of new technologies. Optical schemes are non-invasive, scalable and can be applied to many different systems, but usually have a slow response compared to electrical detection methods. Furthermore, many fluorescent molecules for redox detection degrade in brightness over long exposure times. Here we show that the photoluminescence of pixel arrays of an atomically thin two-dimensional (2D) material, a monolayer of MoS$_{2}$, can image spatial and temporal changes in redox molecule concentration in real time. Because of the strong dependence of MoS$_{2}$ photoluminescence on doping and sensitivity to surface changes characteristic of 2D materials, changes in the local chemical potential significantly modulate the photoluminescence of MoS$_{2}$, with a sensitivity of 0.9 mV/$\sqrt{Hz}$ on a 5 $\mu$m by 5 $\mu$m pixel, corresponding to better than parts-per-hundred changes in redox molecule concentration down to nanomolar concentrations at 100 ms frame rates. The real-time imaging of electrochemical potentials with a fast response time provides a new strategy for visualizing chemical reactions and biomolecules with a 2D material screen.

The MoSeS dynamic omnigami paradigm for smart shape and composition programmable 2D materials.

Abstract: The properties of 2D materials can be broadly tuned through alloying and phase and strain engineering. Shape programmable materials offer tremendous functionality, but sub-micron objects are typically unachievable with conventional thin films. Here we propose a new approach, combining phase/strain engineering with shape programming, to form 3D objects by patterned alloying of 2D transition metal dichalcogenide (TMD) monolayers. Conjugately, monolayers can be compositionally patterned using non-flat substrates. For concreteness, we focus on the TMD alloy MoSe$${}_{2c}$$S$${}_{2(1-c)}$$; i.e., MoSeS. These 2D materials down-scale shape/composition programming to nanoscale objects/patterns, provide control of both bending and stretching deformations, are reversibly actuatable with electric fields, and possess the extraordinary and diverse properties of TMDs. Utilizing a first principles-informed continuum model, we demonstrate how a variety of shapes/composition patterns can be programmed and reversibly modulated across length scales. The vast space of possible designs and scales enables novel material properties and thus new applications spanning flexible electronics/optics, catalysis, responsive coatings, and soft robotics. Current interest in tuning optoelectronic properties of two-dimensional materials focuses on phase and strain engineering. Here the authors propose a novel approach to achieve nanoscale composition/strain patterns and 3D objects with tailored properties using 2D transition metal dicalchogenide alloys.

Spatiotemporal Mapping of Photocurrent in a Monolayer Semiconductor Using a Diamond Quantum Sensor

Abstract: The detection of photocurrents is central to understanding and harnessing the interaction of light with matter. Although widely used, transport-based detection averages over spatial distributions and can suffer from low photocarrier collection efficiency. Here, we introduce a contact-free method to spatially resolve local photocurrent densities using a proximal quantum magnetometer. We interface monolayer MoS2 with a near-surface ensemble of nitrogen-vacancy centers in diamond and map the generated photothermal current distribution through its magnetic field profile. By synchronizing the photoexcitation with dynamical decoupling of the sensor spin, we extend the sensor's quantum coherence and achieve sensitivities to alternating current densities as small as 20 nA per micron. Our spatiotemporal measurements reveal that the photocurrent circulates as vortices, manifesting the Nernst effect, and rises with a timescale indicative of the system's thermal properties. Our method establishes an unprecedented probe for optoelectronic phenomena, ideally suited to the emerging class of two-dimensional materials, and stimulates applications towards large-area photodetectors and stick-on sources of magnetic fields for quantum control.

Low-loss composite photonic platform based on 2D semiconductor monolayers

Abstract: Two dimensional materials such as graphene and transition metal dichalcogenides (TMDs) are promising for optical modulation, detection, and light emission since their material properties can be tuned on-demand via electrostatic doping. The optical properties of TMDs have been shown to change drastically with doping in the wavelength range near the excitonic resonances. However, little is known about the effect of doping on the optical properties of TMDs away from these resonances, where the material is transparent and therefore could be leveraged in photonic circuits. Here, we probe the electro-optic response of monolayer TMDs at near infrared (NIR) wavelengths (i.e. deep in the transparency regime), by integrating them on silicon nitride (SiN) photonic structures to induce strong light$-$matter interaction with the monolayer. We dope the monolayer to carrier densities of ($7.2 \pm 0.8$) $\times$ $10^{13} \textrm{cm}^{-2}$, by electrically gating the TMD using an ionic liquid. We show strong electro-refractive response in monolayer tungsten disulphide (WS$_2$) at NIR wavelengths by measuring a large change in the real part of refractive index $\Delta$n = $0.53$, with only a minimal change in the imaginary part $\Delta$k = $0.004$. The doping induced phase change ($\Delta$n), compared to the induced absorption ($\Delta$k) measured for WS$_2$ ($\Delta$n/$\Delta$k $\sim 125$), a key metric for photonics, is an order of magnitude higher than the $\Delta$n/$\Delta$k for bulk materials like silicon ($\Delta$n/$\Delta$k $\sim 10$), making it ideal for various photonic applications. We further utilize this strong tunable effect to demonstrate an electrostatically gated SiN-WS$_2$ phase modulator using a WS$_2$-HfO$_2$ (Hafnia)-ITO (Indium Tin Oxide) capacitive configuration, that achieves a phase modulation efficiency (V$_\pi$L) of 0.8 V $\cdot$ cm with a RC limited bandwidth of 0.3 GHz.

Composite photonic platform based on 2D semiconductor monolayers

Abstract: We demonstrate phase modulation in the near IR by electrostatically doping 2D semiconductor monolayers integrated on SiN waveguides. We show a $\mathrm{V}_{\pi}\mathrm{L}$ of 1.4 V cm and 0.8 Vcm for MoS 2 and WS 2 , respectively. © 2019 The Author(s)

Diffraction Mapping with a Pixelated Detector to Quantify Crystal Orientation in 3D Structures Made from 2D Materials

Abstract: 1. School of Applied and Engineering Physics, Cornell University, Ithaca, NY, USA 2. Department of Chemistry, University of Chicago, Chicago, IL, USA 3. School of Materials Science and Engineering, Ulsan National Institute of Science and Technology, Ulsan, Republic of Korea 4. James Franck Institute, University of Chicago, Chicago, IL, USA 5. Institute for Molecular Engineering, University of Chicago, Chicago, IL, USA 6. Kavli Institute for Nanoscale Science, Cornell University, Ithaca, NY, USA * Corresponding author: david.a.muller@cornell.edu

Tunable Photocurrent and Photoluminescence from Interlayer Excitons in Twisted Bilayer Graphene and 2D Semiconductors

Abstract: Using ultrafast microscopy we find bound interlayer excitons in twisted bilayer graphene. By quantifying the binding energy, photoluminescence and ultrafast photocurrent we show such bilayer quantum materials enable fast, broadband photosensing.